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Mesoscopic correlations in Tb2Ti2O7 spin liquid

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 Added by Sylvain Petit
 Publication date 2015
  fields Physics
and research's language is English




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We have studied the spin correlations with $bf{k}$= ($frac12$, $frac12$, $frac12$) propagation vector which appear below 0.4, K in tbti spin liquid by combining powder neutron diffraction and specific heat on Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ samples with $x$=0, 0.01, -0.01. The $bf{k}$= ($frac12$, $frac12$, $frac12$) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1),K. Refining the subtracted patterns at 0.07,K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 mub ordered on a length scale of about 20 AA. In addition, long range order involving a small spin component of 0.1 to 0.2 mub is detected for the $x$= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ($frac12$, $frac12$, $frac12$) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.



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We report time-of-flight neutron scattering measurements of the magnetic spectrum of Tb3+ in Tb2Ti2O7. The data, which extend up to 120 meV and have calibrated intensity, enable us to consolidate and extend previous studies of the single-ion crystal field spectrum. We successfully refine a model for the crystal field potential in Tb2Ti2O7 without relying on data from other rare earth titanate pyrochlores, and we confirm that the ground state is a non-Kramers doublet with predominantly |+/-4> components. We compare the model critically with earlier models.
Neutron scattering experiments on a polycrystalline sample of the frustrated pyrochlore magnet Tb2Ti2O7, which does not show any magnetic order down to 50 mK, have revealed that it shows condensation behavior below 0.4 K from a thermally fluctuating paramagnetic state to a spin-liquid ground-state with quantum spin fluctuations. Energy spectra change from quasielastic scattering to a continuum with a double-peak structure at energies of 0 and 0.8 K in the spin-liquid state. Specific heat shows an anomaly at the crossover temperature.
High resolution time-of-flight neutron scattering measurements on Tb2Ti2O7 reveal a rich low temperature phase diagram in the presence of a magnetic field applied along [110]. In zero field at T=0.4 K, terbium titanate is a highly correlated cooperative paramagnet with disordered spins residing on a pyrochlore lattice of corner-sharing tetrahedra. Application of a small field condenses much of the magnetic diffuse scattering, characteristic of the disordered spins, into a new Bragg peak characteristic of a polarized paramagnet. At higher fields, a magnetically ordered phase is induced, which supports spin wave excitations indicative of continuous, rather than Ising-like spin degrees of freedom.
We combine two aspects of magnetic frustration, multiferroicity and emergent quasi-particles in spin liquids, by studying magneto-electric monopoles. Spin ice offers to couple these emergent topological defects to external fields, and to each other, in unusual ways, making possible to lift the degeneracy underpinning the spin liquid and to potentially stabilize novel forms of charge crystals, opening the path to a magnetic crystallography. In developing the general phase diagram including nearest-neighbour coupling, Zeeman energy, electric and magnetic dipolar interactions, we uncover the emergence of a bi-layered crystal of singly-charged monopoles, whose stability, remarkably, is strengthened by an external [110] magnetic field. Our theory is able to account for the ordering process of Tb2Ti2O7 in large field for reasonably small electric energy scales.
We present a comprehensive analysis of high resolution neutron scattering data involving Neutron Spin Echo spectroscopy and Spherical Polarimetry which confirm the first order nature of the helical transition and reveal the existence of a new spin liquid skyrmion phase. Similar to the blue phases of liquid crystals this phase appears in a very narrow temperature range between the low temperature helical and the high temperature paramagnetic phases.
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